A series of ferrocenylaldimines (Fc-CH=N-R) has been prepared by Schiff base condensation of formylferrocene with polyacenylamines RNH/sub 2/ where R= naphthyl, 5,6,7,8-tetrahydronaphthyl, anthracenyl, and pyrenyl groups. This step was followed by oxidation with TCNQ to give(Fc-CH=N-R)(TCNQ)/sub 2/ salts. The electronic state of iron in these compounds was investigated by means of /sup 57/Fe Mossbauer spectroscopy.